CN115477810A - Spraying-free polypropylene material and preparation method thereof - Google Patents
Spraying-free polypropylene material and preparation method thereof Download PDFInfo
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- CN115477810A CN115477810A CN202211123177.1A CN202211123177A CN115477810A CN 115477810 A CN115477810 A CN 115477810A CN 202211123177 A CN202211123177 A CN 202211123177A CN 115477810 A CN115477810 A CN 115477810A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/10—Homopolymers or copolymers of propene
- C08L23/12—Polypropene
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/08—Metals
- C08K2003/0812—Aluminium
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/08—Metals
- C08K2003/0862—Nickel
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/01—Magnetic additives
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Abstract
The invention discloses a spraying-free polypropylene material and a preparation method thereof, wherein the spraying-free polypropylene material comprises the following components in parts by weight: 50-95 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 0.1-10 parts of magnetically attractable powder and 1.25-35 parts of functional auxiliary agent, wherein no magnetic attraction force exists between the magnetically attractable powder and an iron part. Meanwhile, the invention also discloses a preparation method of the spray-free polypropylene material. The surface of the spraying-free polypropylene material provided by the invention has a magnetic attraction characteristic, so that the use of an adhesive can be avoided when a swing part is placed, and the requirement for personalized quick replacement is met.
Description
Technical Field
The invention belongs to the technical field of plastic materials, and particularly relates to a spraying-free polypropylene material and a preparation method thereof.
Background
The polypropylene material is applied to a plurality of fields such as household appliances, automobiles and the like. In some application scenes of appearance parts such as shells or interior trim parts, users not only want the appearance parts to have good appearance effects, but also have the requirements of pasting personalized stickers and fixedly placing personalized ornament parts, such as placing ornament parts such as aromatherapy, pet toys and the like on an automobile instrument panel.
The current mode of fixing of sticker and goods of furniture for display rather than for use mainly is gluing through gluing agent, but uses sticky mode to have following several problems: (1) The requirement on the cleanness degree of the bonding surface is high, so that a good fixing effect can be achieved; (2) Because the surface energy of PP is not high and the PP belongs to a material difficult to adhere, the PP is easy to fall off after being adhered for a long time; (3) The use of the adhesive can bring air pollution in a small space and aggravate the condition of bad smell in the vehicle; (4) The adhesive connection scheme is not easy to replace, and adhesive residues are easy to remain during replacement, so that great adverse effects are brought to the appearance.
Disclosure of Invention
The invention provides a spraying-free polypropylene material and a preparation method thereof, aiming at the problem that a polypropylene part made of the existing polypropylene material is not easy to be connected and fixed with a decoration.
The technical scheme adopted by the invention for solving the technical problems is as follows:
on one hand, the embodiment of the invention provides a spraying-free polypropylene material, which comprises the following components in parts by weight: 50-95 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 0.1-10 parts of magnetically attractable powder and 1.25-35 parts of functional auxiliary agent, wherein no magnetic attraction force exists between the magnetically attractable powder and an iron part.
Optionally, the spray-free polypropylene material comprises the following components by weight: 60-90 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 1-10 parts of magnetically attractable powder and 1.3-30 parts of functional auxiliary agent.
Optionally, the melt flow rate of the polypropylene resin is 12-45g/10min at 230 ℃ and under the condition of 2.16 kg.
Optionally, the magnetically attractable powder includes ferromagnetic particles and/or ferromagnetic particles coated with a polymer, and the ferromagnetic particles include one or more of metal powder, metal oxide, iron sulfide, and alloy.
Optionally, the metal powder comprises one or more of Fe, co and Ni; the metal oxide comprises Co 3 O 4 And NiO; the alloy includes one or more of Fe-Pt, al-Ni, and Ni-C.
Optionally, the polymer comprises one or more of polyethylene, polypropylene, polyacrylate, and polystyrene.
Optionally, the magnetically attractable powder has a particle size range of 0.01-100 μm.
Optionally, the metallic appearance filler comprises one or more of metal powder, pearlescent pigment, aluminum powder, aluminum water pigment, mica pearlescent pigment.
Optionally, on the basis of the weight of the spray-free polypropylene material, the functional additive comprises the following components in parts by weight: 0-20 parts of filler, 1-10 parts of toughening agent, 0.1-0.5 part of coupling agent, 0.05-2 parts of antioxidant, 0.05-2 parts of light stabilizer and 0.05-0.5 part of metal ion passivator.
Optionally, the filler comprises one or more of talc, calcium carbonate, barium sulfate, wollastonite, and short glass fibers;
the toughening agent comprises one or more of an ethylene-octene copolymer and an ethylene-butene copolymer;
the coupling agent comprises one or more of titanate coupling agent and silane coupling agent;
the antioxidant comprises one or more of amine antioxidant, phenol antioxidant, phosphite antioxidant and sulfur-containing antioxidant;
the light stabilizer comprises one or more of hindered amine light stabilizer, salicylic acid light stabilizer, benzophenone light stabilizer and benzotriazole light stabilizer;
the metal ion passivator comprises one or more of a bis-salicylidene diamine passivator and an oxamide passivator.
On the other hand, the invention also provides a preparation method of the spraying-free polypropylene material, wherein the functional auxiliary agent comprises a filler, a toughening agent, a coupling agent, an antioxidant, a light stabilizer and a metal ion passivator, and the preparation method comprises the following steps:
mixing a filler, a metal appearance filler, magnetically attractable powder and a coupling agent to obtain a mixed magnetically attractable pigment filler;
mixing the mixed magnetic pigment filler with part of the polypropylene resin, and extruding and granulating by using a double-screw extruder to obtain magnetic masterbatch;
and mixing the magnetic attraction color master batch with the rest of the polypropylene resin, the toughening agent, the antioxidant, the light stabilizer and the metal ion passivator, and extruding and granulating by using a double-screw extruder to obtain the spray-free polypropylene material.
Optionally, the extrusion granulation conditions are as follows: the temperature of the T1 area is 70-120 ℃, the temperature from T2 to the machine head is 160-210 ℃, and the rotating speed of the screw is 400-800r/min.
In the invention, the spraying-free polypropylene material can realize good appearance effect without a spraying process, reduce the spraying procedure and improve the environmental protection and the recyclability of the product. And exempt from the spraying polypropylene material, make the finished piece surface of preparation possess magnetism and inhale the characteristic, when the user needs attach or place individualized goods of furniture for display rather than for use or chartlet at polypropylene products, can avoid using the gluing agent, paste soon and take off soon, satisfy individualized quick replacement's demand. Compared with the traditional polypropylene composite material, the spraying-free polypropylene material disclosed by the invention has the advantages that the magnetically attractable powder is used, the magnetically attractable powder and the iron part have no magnetic attraction, the magnetically attractable powder is prevented from migrating to the surface layer of the part, the appearance and the functionality of the part are endowed, and more requirements of a user on the finished part can be met.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects solved by the present invention more clear, the present invention is further described in detail below with reference to the embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The embodiment of the invention discloses a spraying-free polypropylene material, which comprises 50-95 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 0.1-10 parts of magnetically attractable powder and 1.25-35 parts of functional auxiliary agent, wherein no magnetic attraction exists between the magnetically attractable powder and an iron part.
In this embodiment, exempt from to spout coating polypropylene material and can not realize good outward appearance effect through spraying process, reduce the process of spraying paint, promote the feature of environmental protection and the recyclability of product. And exempt from the spraying polypropylene material, make the finished piece surface of preparation possess magnetism and inhale the characteristic, when the user needs attach or place individualized goods of furniture for display rather than for use or chartlet at polypropylene products, can avoid using the gluing agent, paste soon and take off soon, satisfy individualized quick replacement's demand. Compared with the traditional polypropylene composite material, the spraying-free polypropylene material disclosed by the invention has the advantages that the magnetically attractable powder is used, the magnetically attractable powder and the iron part have no magnetic attraction, the magnetically attractable powder is prevented from migrating to the surface layer of the part, the appearance and the functionality of the part are endowed, and more requirements of a user on the finished part can be met.
In a preferred embodiment, the spray-free polypropylene material comprises the following components by weight: 60-90 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 1-10 parts of magnetically attractable powder and 1.3-30 parts of functional auxiliary agent.
In some embodiments, the polypropylene resin has a melt flow rate of 12 to 45g/10min at 230 ℃ under 2.16 kg. The melt flow rate of the polypropylene resin is 12 to 45g/10min, which is advantageous for dispersion of the filler and improvement of appearance quality, and within this range, the filler is more easily dispersed as the melt flow rate increases. However, when the melt flow rate exceeds 45g/10min, the mechanical property of the product prepared by the spray-free polypropylene material is poor. However, when the melt flow rate is less than 12g/10min, the filler is not easy to disperse, and the appearance quality of the product is affected. Specifically, the melt flow rate may be 14g/10min, 18g/10min, 22g/10min, 25g/10min, 28g/10min, 30g/10min, 35g/10min, 40g/10min, or the like.
In some embodiments, the magnetically attractable powder includes ferromagnetic particles and/or polymer-encapsulated ferromagnetic particles, the ferromagnetic particles including one or more of metal powders, metal oxides, iron sulfides, and alloys. In particular, the ferromagnetic particles are micro-or nano-scale particles.
In some embodiments, the metal powder comprises one or more of Fe, co, and Ni; the metal oxide comprises Co 3 O 4 And NiO; the alloy includes one or more of Fe-Pt, al-Ni, and Ni-C.
The magnetic permeability of the magnetically attractable powder is relatively low, and no magnetic attraction exists between the magnetically attractable powder and a ferrous part. Because the injection molding or extrusion equipment for spraying-free polypropylene materials is mainly iron equipment, the magnetic conductivity is too high, and magnetic powder can be attracted to migrate to the surface layer of a workpiece due to the attraction of the iron equipment, so that the surface filler of the workpiece is concentrated, the thermal expansion coefficient difference between the surface layer and the inner layer of the workpiece is easy to be too large, the workpiece is warped and deformed, and the process control difficulty is increased. Meanwhile, the magnetic powder can be easily adsorbed on the inner wall of the screw or the charging barrel, so that the service life of the device is shortened. In addition, the magnetically attractable powder generally has a certain color, and if the magnetically attractable powder is too concentrated on the surface layer of the workpiece, the color of the magnetically attractable powder may cause too much interference to the appearance of the workpiece, thereby shielding the color development effect of the toner and affecting the spraying-free appearance effect. Therefore, the magnetically attractable powder with relatively low magnetic permeability is selected to avoid the magnetically attractable powder from migrating to the surface layer of the workpiece when the spraying-free polypropylene material is subjected to injection molding.
In some embodiments, the polymer comprises one or more of polyethylene, polypropylene, polyacrylate, and polystyrene.
In some embodiments, the magnetically attractable powder has a particle size in a range of 0.01-100 μm. By controlling the particle size of the magnetically attractable powder, the adverse effect of overlarge particle size on the appearance of a workpiece can be avoided. Specifically, the particle size of the magnetically attractable powder may be 0.01 μm, 5 μm, 10 μm, 25 μm, 30 μm, 50 μm, 60 μm, 70 μm, 100 μm, or the like.
In some embodiments, the metallic appearance filler comprises one or more of metal powder, pearlescent pigment, aluminum powder, aluminum water pigment, mica pearlescent pigment.
In some embodiments, the functional aid comprises the following components by weight, based on the weight of the spray-free polypropylene material: 0-20 parts of filler, 1-10 parts of toughening agent, 0.1-0.5 part of coupling agent, 0.05-2 parts of antioxidant, 0.05-2 parts of light stabilizer and 0.05-0.5 part of metal ion passivator.
In a preferred embodiment, based on the weight of the spray-free polypropylene material, the functional assistant comprises the following components in parts by weight: 0-15 parts of filler, 1-10 parts of toughening agent, 0.1-0.5 part of coupling agent, 0.05-2 parts of antioxidant, 0.05-2 parts of light stabilizer and 0.1-0.5 part of metal ion passivator. The metal ions play a role in catalyzing the photodegradation of the polypropylene material, and the adverse effect of the metal ions introduced by the magnetically attractable powder on the weather resistance of the polypropylene can be eliminated by adding the metal ion passivator.
In some embodiments, the filler comprises one or more of talc, calcium carbonate, barium sulfate, wollastonite, and short glass fibers.
The toughening agent includes one or more of an ethylene-octene copolymer and an ethylene-butene copolymer.
The coupling agent comprises one or more of a titanate coupling agent and a silane coupling agent.
The antioxidant comprises one or more of amine antioxidant, phenol antioxidant, phosphite antioxidant and sulfur-containing antioxidant.
The light stabilizer comprises one or more of hindered amine light stabilizer, salicylic acid light stabilizer, benzophenone light stabilizer and benzotriazole light stabilizer.
The metal ion passivator comprises one or more of a bis-salicylidene diamine passivator and an oxamide passivator.
On the other hand, an embodiment of the present invention further provides a preparation method of the above spray-free polypropylene material, including the following steps:
and mixing the filler, the metal appearance filler, the magnetically attractable powder and the coupling agent to obtain the mixed magnetically attractable pigment filler.
And mixing the mixed magnetically attractable pigment filler with part of the polypropylene resin, and extruding and granulating by using a double-screw extruder to obtain the magnetically attractable color master batch.
And mixing the magnetically attractable color master batch with the rest of the polypropylene resin, the toughening agent, the antioxidant, the light stabilizer and the metal ion passivator, and extruding and granulating by using a double-screw extruder to obtain the spray-free polypropylene material.
In some embodiments, the extrusion granulation conditions are: the temperature of the T1 area is 70-120 ℃, the temperature from T2 to the machine head is 160-210 ℃, and the rotating speed of the screw is 400-800r/min.
The present invention is further illustrated by the following examples.
Example 1
This example is used to illustrate the spray-free polypropylene material and the preparation method thereof disclosed in the present invention, and includes the following steps:
10 parts of 1250-mesh talcum powder (filling agent), 2 parts of waterborne aluminum paste (Al 60 percent has the average particle size of 50 mu m), 3 parts of carbonyl micron Fe powder (magnetically attractable powder) and 0.1 part of titanate coupling agent are mixed and put into a high-speed mixer for premixing for 5min at the rotating speed of 1000rpm to obtain the mixed magnetically attractable pigment filler. The average particle size of the carbonyl micrometer Fe powder is 10 μm.
And mixing the obtained mixed magnetically attractable pigment filler with 40 parts of polypropylene resin, and extruding and granulating by using a double-screw extruder to obtain the magnetically attractable color master batch. Wherein the temperature of the T1 area is 100 ℃, the temperature of T2 is 180 ℃ of the machine head, and the rotating speed of the screw is 600r/min. The melt flow rate of the polypropylene resin was 12g/10min at 230 ℃ under 2.16 kg.
Mixing magnetically attractable color master batch with 40 parts of polypropylene resin, 5 parts of ethylene-octene copolymer (toughening agent), 0.05 part of compound of phenolic antioxidant and phosphorous acid antioxidant, 0.05 part of hindered amine light stabilizer and 0.1 part of metal ion passivator (Pasteur Irganox MD 1024), and extruding and granulating by using a double-screw extruder to obtain the spray-free polypropylene material.
Wherein the temperature of the T1 area is 100 ℃, the temperature of T2 is 180 ℃ of the machine head, and the rotating speed of the screw is 600r/min. The melt flow rate of the toughening agent is 4.8g/10min at 230 ℃ and 2.16 kg.
Example 2
In this example, which includes most of the operating steps in example 1, the polypropylene resin is 75 parts, 5 parts of pearl powder is used instead of aqueous aluminum paste, and 5 parts of Ni-C powder is used instead of carbonyl micron Fe powder, unlike example 1. The average particle size of the pearl powder was 180 μm, and the average particle size of the Ni-C powder was 50 μm.
Example 3
In this example, including most of the operation steps in example 1, unlike example 1, 75 parts of polypropylene resin, 1 part of pearl powder was used instead of aqueous aluminum paste, 4 parts of ethylene-octene copolymer, and 10 parts of carbonyl micrometer Fe powder. The melt flow rate of the polypropylene resin was 35g/10min at 230 ℃ under 2.16 kg. The average particle size of the pearl powder was 180. Mu.m.
Example 4
In this example, which includes most of the operating steps in example 1, unlike example 1, no metal ion passivator is included: basf IrganoxMD1024.
Example 5
In this example, including most of the operation steps in example 1, the melt flow rate of the polypropylene resin was 45g/10min at 230 ℃ under 2.16kg, unlike example 1.
Example 6
In this example, including most of the operation steps in example 1, the melt flow rate of the polypropylene resin was 25g/10min at 230 ℃ under 2.16kg, unlike example 1.
Comparative example 1
In this comparative example, which includes most of the operation steps in example 2, unlike example 2, fe was used 3 O 4 5 parts of powder replaces Ni-C powder. Fe 3 O 4 The average particle size of the powder was 50 μm.
Comparative example 2
In this comparative example, which includes most of the operation steps in example 1, the melt flow rate of the polypropylene resin was 9g/10min at 230 ℃ under 2.16kg, unlike example 1.
Comparative example 3
In this comparative example, which includes most of the operation steps in example 1, the melt flow rate of the polypropylene resin was 50g/10min at 230 ℃ under 2.16kg, unlike example 1.
Performance testing
The spray-free polypropylene materials prepared in the above examples 1 to 6 and comparative examples 1 to 3 were injection molded into articles and tested for properties.
The tensile strength is tested according to GB/T1040.2-2018, and the notched Izod impact strength is tested according to GB/T1843-2008. The magnetic attraction was evaluated by measuring the vertical pulling force using a commercially available neodymium boron magnet in combination with a tensile machine. The appearance effect was visually evaluated.
The results of the tests are shown in Table 1.
TABLE 1
From the test results of examples 1-6 and comparative examples 2-3, it can be seen that by changing the melt flow rate of polypropylene, the appearance quality and mechanical properties of the spray-free polypropylene material product can be affected. It can be known from the test results of examples 1 to 3 and comparative example 1 that, by selecting the magnetic powder with higher magnetic permeability, although the vertical pulling-out force of the workpiece is higher, the magnetic powder migrates to the surface layer of the workpiece, and the color of the magnetic powder body has obvious influence on the appearance effect, thereby causing bad spraying-free appearance effect.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (12)
1. The spraying-free polypropylene material is characterized by comprising the following components in parts by weight: 50-95 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 0.1-10 parts of magnetically attractable powder and 1.25-35 parts of functional auxiliary agent, wherein no magnetic attraction force exists between the magnetically attractable powder and an iron part.
2. The spray-free polypropylene material according to claim 1, comprising the following components by weight: 60-90 parts of polypropylene resin, 0.1-5 parts of metal appearance filler, 1-10 parts of magnetically attractable powder and 1.3-30 parts of functional auxiliary agent.
3. The spray-free polypropylene material according to claim 1, wherein the melt flow rate of the polypropylene resin is 12-45g/10min at 230 ℃ and 2.16 kg.
4. The spray-free polypropylene material of claim 1, wherein the magnetically attractable powder comprises ferromagnetic particles and/or polymer-coated ferromagnetic particles, and the ferromagnetic particles comprise one or more of metal powder, metal oxide, iron sulfide, and alloy.
5. The spray-free polypropylene material of claim 4, wherein the metal powder comprises one or more of Fe, co and Ni; the metal oxide comprises Co 3 O 4 And NiO; the alloy includes one or more of Fe-Pt, al-Ni, and Ni-C.
6. The spray-free polypropylene material of claim 4, wherein the polymer comprises one or more of polyethylene, polypropylene, polyacrylate, and polystyrene.
7. The spray-free polypropylene material of claim 4, wherein the magnetically attractable powder has a particle size of 0.01-100 μm.
8. The spray-free polypropylene material according to claim 1, wherein the metallic appearance filler comprises one or more of metal powder, pearlescent pigment, aluminum powder, aluminum water pigment, mica pearlescent pigment.
9. The spray-free polypropylene material according to claim 1, wherein the functional additives comprise the following components by weight, based on the weight of the spray-free polypropylene material: 0-20 parts of filler, 1-10 parts of toughening agent, 0.1-0.5 part of coupling agent, 0.05-2 parts of antioxidant, 0.05-2 parts of light stabilizer and 0.05-0.5 part of metal ion passivator.
10. The spray-free polypropylene material of claim 9, wherein the filler comprises one or more of talc, calcium carbonate, barium sulfate, wollastonite, and short glass fibers;
the toughening agent comprises one or more of an ethylene-octene copolymer and an ethylene-butene copolymer;
the coupling agent comprises one or more of titanate coupling agent and silane coupling agent;
the antioxidant comprises one or more of amine antioxidant, phenol antioxidant, phosphite antioxidant and sulfur-containing antioxidant;
the light stabilizer comprises one or more of hindered amine light stabilizer, salicylic acid light stabilizer, benzophenone light stabilizer and benzotriazole light stabilizer;
the metal ion passivator comprises one or more of a bis-salicylidene diamine passivator and an oxamide passivator.
11. The preparation method of the spray-free polypropylene material as claimed in any one of claims 1 to 10, wherein the functional additives comprise a filler, a toughening agent, a coupling agent, an antioxidant, a light stabilizer and a metal ion passivator, and the preparation method comprises the following steps:
mixing a filler, a metal appearance filler, magnetically attractable powder and a coupling agent to obtain a mixed magnetically attractable pigment filler;
mixing the mixed magnetically attractable pigment filler with part of the polypropylene resin, and performing extrusion granulation by using a double-screw extruder to obtain magnetically attractable color master batch;
and mixing the magnetic attraction color master batch with the rest of the polypropylene resin, the toughening agent, the antioxidant, the light stabilizer and the metal ion passivator, and extruding and granulating by using a double-screw extruder to obtain the spray-free polypropylene material.
12. The method according to claim 11, wherein the conditions for extrusion granulation are: the temperature of the T1 area is 70-120 ℃, the temperature from T2 to the machine head is 160-210 ℃, and the rotating speed of the screw is 400-800r/min.
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CN114702533A (en) * | 2022-03-31 | 2022-07-05 | 金发科技股份有限公司 | Benzoate monomer containing ferrocene unit and preparation method thereof |
CN114702533B (en) * | 2022-03-31 | 2024-03-22 | 金发科技股份有限公司 | Benzoate monomer containing ferrocene unit and preparation method thereof |
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